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Iron and nitrogen co-doped carbon-oxygen reduction catalyst, and preparation method and application thereof

A co-doping and catalyst technology, applied in structural parts, electrical components, battery electrodes, etc., can solve the problems of unfavorable reactant and product mass transfer, metal nanoparticles precipitation and agglomeration, reduction of active site utilization, etc. The reduction catalytic activity and electrochemical stability are excellent, the preparation method is simple, and the effect of the optimization of the preparation method

Active Publication Date: 2018-12-28
BEIJING UNIV OF CHEM TECH
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  • Summary
  • Abstract
  • Description
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Problems solved by technology

However, the pore structure of TM-N-C catalysts prepared by pyrolysis of single metal (Co or Zn) ZIF is mainly micropores, which is not conducive to the mass transfer of reactants and products, and the ZIF structure is easy to collapse during the pyrolysis process, resulting in a decrease in the specific surface area. On the other hand, during the pyrolysis process, metal nanoparticles are prone to precipitation and agglomeration, and some active sites are buried in the three-dimensional carbon skeleton, and the utilization rate of active sites is reduced.

Method used

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  • Iron and nitrogen co-doped carbon-oxygen reduction catalyst, and preparation method and application thereof
  • Iron and nitrogen co-doped carbon-oxygen reduction catalyst, and preparation method and application thereof
  • Iron and nitrogen co-doped carbon-oxygen reduction catalyst, and preparation method and application thereof

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Embodiment 1

[0037] Using Fe, Zn-ZIF as a precursor for high-temperature pyrolytic carbonization to prepare an iron-nitrogen co-doped carbon oxygen reduction catalyst includes the following steps:

[0038] (1) Zn(NO 3 ) 2 ·6H 2 O (788.31 mg, 2.38 mmol) and FeSO 4 ·7H 2 O (33.1 mg, 0.12 mmol) was dissolved in 90 mL of methanol, while benzimidazole (1180 mg, 10 mmol) was dissolved in 90 mL of methanol, ultrasonically dissolved and dispersed evenly, and the benzimidazole containing The methanol solution is poured into the methanol solution of the metal salt, and the solution mixing rate is 9mL s -1 ; Stir at room temperature for 1 min after mixing, pour into a 200 mL reaction kettle, and then transfer to an oven at 130 o C for 24 h, cooling, suction filtration and repeated washing with organic solvents, and then drying to obtain a yellow powder. Among them, Zn(NO 3 ) 2 ·6H 2 O and FeSO 4 ·7H 2 O molar ratio is 20, metal salt and benzimidazole molar ratio is 0.25, and the concentrat...

Embodiment 2

[0042] The preparation process was similar to that of Example 1, except that the hydrothermal reaction time was reduced to 16 h during the preparation of the precursor Fe,Zn-ZIF. SEM image ( Figure 7 ) shows that the prepared Fe,Zn-ZIF has a cylindrical shape with an average diameter of about 6.5 μm, and the oxygen reduction performance test of the catalyst prepared by pyrolytic carbonization ( Figure 8 ) shows that the catalyst has better electrocatalytic activity than commercial 20%Pt / C, and the half-wave potential exceeds 40 mV, which is about 10 mV lower than that in Example 1.

Embodiment 3

[0044] A preparation process similar to that of Example 1 was adopted, except that, in the preparation process of the precursor Fe, Zn-ZIF, the molar ratio of metal salt to benzimidazole was 0.125. SEM image ( Figure 9 ) shows that the morphology of the prepared Fe, Zn-ZIF is cylindrical, and the aspect ratio is reduced from 1:1 to 1:2. The oxygen reduction performance test of the catalyst prepared by pyrolysis carbonization ( Figure 10 ) shows that the catalyst has better electrocatalytic activity than commercial 20% Pt / C, and the half-wave potential exceeds 35 mV, which is about 15 mV lower than that in Example 1.

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Abstract

The invention relates to an iron and nitrogen co-doped carbon-oxygen reduction catalyst, and a preparation method and application thereof. Fe / Zn bimetallic ZIF with elemental gradient distribution isprepared to prepare an iron and nitrogen co-doped carbon-oxygen reduction catalyst by pyrolysis and carbonization as a precursor, in order to improve the utilization rate of active sites, optimize thepore structure and further enhance the catalytic activity. The iron and nitrogen co-doped carbon-oxygen reduction catalyst prepared by the invention can efficiently catalyze the oxygen reduction reaction and exhibits better oxygen reduction catalytic activity and electrochemical stability than the commercial Pt / C catalyst. The preparation method is simple and controllable, has short cycle, abundant raw material reserves and low cost, and can realize large-scale production.

Description

technical field [0001] The invention belongs to the technical field of catalyst preparation, in particular to an iron and nitrogen co-doped carbon oxygen reduction catalyst and its preparation method and application, especially to an iron / zinc bimetallic organic framework material (MOFs) with element gradient distribution as Precursor iron and nitrogen co-doped carbon oxygen reduction catalyst and its application. Background technique [0002] Due to its advantages of environmental protection and high efficiency, fuel cells are considered to be one of the most potential energy conversion devices in the fields of electric vehicles, stationary power stations and portable power supplies. The energy barrier of the fuel cell cathode oxygen reduction reaction is relatively high, and an efficient catalyst is required to reduce the activation energy of the reaction and increase the reaction rate. At present, noble metal platinum-based catalysts are widely used in the oxygen reducti...

Claims

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Application Information

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IPC IPC(8): H01M4/90
CPCH01M4/90H01M4/9041Y02E60/50
Inventor 王峰郭志远窦美玲宋夜张正平李志林
Owner BEIJING UNIV OF CHEM TECH
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